I'm surprised so many people have mention System Shock 2, but only 3 have mentioned Thief, also by Looking Glass.
I found Thief much scarier than SS2, especially the level "Return to the Haunted Cathedral." The sounds the undead made were very creepy - the moaning of the zombies, the backwards laughter and whispering of the Haunts (Flames, flames, nothing but flames! Join us, join us, join us now!) and the backwards speech of the apparitions. The fact that your character wasn't a very good fighter and could die very easily also gave a sense of mortailty you don't have in many first-person games, which also contributed to the scariness.
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I'm not lazy, I'm "motivationally challenged."
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